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Wettability of Quartz Surfaces Under Carbon Dioxide Geo-Sequestration Conditions

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Edith Cowan University Research Online Theses: Doctorates and Masters Theses 2019 Wettability of quartz surfaces under carbon dioxide geo- sequestration conditions. A theoretical study Aleksandr Abramov Edith Cowan University Follow this and additional works at: https://ro.ecu.edu.au/theses Part of the Engineering Commons Recommended Citation Abramov, A. (2019). Wettability of quartz surfaces under carbon dioxide geo-sequestration conditions. A theoretical study. https://ro.ecu.edu.au/theses/2232 This Thesis is posted at Research Online. https://ro.ecu.edu.au/theses/2232 Edith Cowan University Copyright Warning You may print or download ONE copy of this document for the purpose of your own research or study. The University does not authorize you to copy, communicate or otherwise make available electronically to any other person any copyright material contained on this site. You are reminded of the following: Copyright owners are entitled to take legal action against persons who infringe their copyright. A reproduction of material that is protected by copyright may be a copyright infringement. Where the reproduction of such material is done without attribution of authorship, with false attribution of authorship or the authorship is treated in a derogatory manner, this may be a breach of the author’s moral rights contained in Part IX of the Copyright Act 1968 (Cth). Courts have the power to impose a wide range of civil and criminal sanctions for infringement of copyright, infringement of moral rights and other offences under the Copyright Act 1968 (Cth). Higher penalties may apply, and higher damages may be awarded, for offences and infringements involving the conversion of material into digital or electronic form. Wettability of Quartz Surfaces under Carbon Dioxide Geo-Sequestration Conditions. A Theoretical Study Aleksandr Abramov Submitted for the Degree of Doctor of Philosophy Edith Cowan University School of Engineering 2019 Abstract The wettability of rocks under reservoir conditions is important to ensure and secure long term underground storage of carbon dioxide. The composition of those rocks vary significantly and are influenced by the fact that quartz is the second most abundant mineral in the earth's continental crust. Thus, the CO2 wettability of quartz dominates the overall CO2 trapping performance of storage and cap rocks. If depleted oil or gas reservoirs are used for storage of CO2 quartz surfaces of rocks in reservoirs which have been previously exposed to hydrocarbons might be covered with chemisorpt hydrocarbon molecules. The CO2 wettability of these chemically modified quartz is studied in this work with molecular dynamics. To model quartz surfaces with chemisorpt hydrocarbons both CLAYFF and DREIDING force fields are coupled at atomic site charge level using the density functional theory and the Bader charge analysis. Augmented with modified charges of the OC bond, CLAYFF and the DREIDING force fields are applied to solve the practical problem of calculating the contact angle of a water droplet on alkylated quartz surfaces in a CO2 environment. A systematic computational study of wettability of fully hydroxylated and alkylated (001) -quartz surface in carbon dioxide atmosphere with respect to surface concentration of pentyl groups is performed. Alkylated quartz surfaces have been shown to be extremely hydrophobic even when the surface density of hydroxyl groups is close to the highest naturally observed. The study also verifies that a comprehensive description of wettability of alkylated quartz surface requires three parameters: the theoretical contact angle, the apparent contact angle and the hidden contact angle. These contact angles are determined at the tip level of pentyl groups and the level of the quartz surface. The hidden contact angle is calculated as the angle of a water "skirt", which is formed between the level of the quartz surface and the tip level of pentyl groups. Additionally, the concept and the method of how to determine computational contact angles of a liquid droplet resting on a solid surface from individual snapshots of molecular dynamics simulations have been formulated, implemented and analysed in this work. Spherical coordinates to circumscribe a sphere around given configuration of water molecules form the basis of the method, which is thus natural and consistent with the droplet's geometric computational framework. 2 Declaration I certify that this thesis does not, to the best of my knowledge and belief: i. incorporate without acknowledgment any material previously submitted for a degree or diploma in any institution of higher education; ii. contain any material previously published or written by another person except where due reference is made in the text of this thesis; or iii. contain any defamatory material. Aleksandr Abramov 27/07/2019 3 Acknowledgments This work was supported by Edith Cowan University Petroleum Engineering PhD Scholarship and by resources provided by the Pawsey Supercomputing Centre with funding from the Australian Government and the Government of Western Australia. 4 Table of Contents List of tables ................................................................................................................................ 8 List of figures .............................................................................................................................. 9 1. Introduction....................................................................................................................... 22 1.1. Scope and objective ................................................................................................... 22 1.2. Methods, procedures and process ............................................................................ 22 1.3. Results, observations and conclusions ...................................................................... 22 1.4. Novel and additive information ................................................................................. 22 1.5. Thesis organization .................................................................................................... 23 1.6. Publications ................................................................................................................ 23 2. Literature review ............................................................................................................... 25 2.1. Global warming .......................................................................................................... 25 2.1.1. Overview ............................................................................................................. 25 2.1.2. Response strategies ............................................................................................ 29 2.2. Carbon capture and storage ...................................................................................... 30 2.2.1. Overview ............................................................................................................. 30 2.2.2. Carbon geo-sequestration projects .................................................................... 32 2.3. Wettability and carbon dioxide storage capacity of rocks ........................................ 34 2.4. Properties of carbon dioxide in geological conditions .............................................. 37 2.5. Quartz wettability in presence of carbon dioxide ..................................................... 40 2.5.1. Experimental studies .......................................................................................... 41 2.5.2. Theoretical studies ............................................................................................. 47 2.6. Quartz crystal ............................................................................................................. 49 2.7. Quartz surface ............................................................................................................ 51 2.8. Conclusions ................................................................................................................ 56 3. Computational methods ................................................................................................... 57 5 3.1. Overview .................................................................................................................... 57 3.2. Force fields ................................................................................................................. 57 3.3. Molecular dynamics ................................................................................................... 63 3.4. Density functional theory .......................................................................................... 67 3.5. Conclusions ................................................................................................................ 69 4. The suitability of spheroidal constructions to estimate the contact angle using snapshots of molecular dynamics simulations .......................................................................................... 71 4.1. Annotation ................................................................................................................. 71 4.2. Introduction and motivation ..................................................................................... 71 4.3. Method development ................................................................................................ 73 4.4. Computational details ...............................................................................................
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